Solar Fuel Synthesis Using a Semiartificial Colloidal Z-Scheme

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(43), С. 29865 - 29876

Опубликована: Окт. 16, 2024

The integration of enzymes with semiconductor light absorbers in semiartificial photosynthetic assemblies offers an emerging strategy for solar fuel production. However, such colloidal biohybrid systems rely currently on sacrificial reagents, and semiconductor-enzyme powder that couple production to water oxidation are therefore needed mimic overall reaction. Here, we present a Z-scheme enzyme system produces electrons sourced from water. This "closed-cycle" approach utilizes particulate SrTiO

Язык: Английский

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Photocatalytic hydrogen evolution and simultaneously converting high-concentration of thiols into disulfides with excellent yield under visible-light

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(6), С. 2726 - 2736

Опубликована: Янв. 1, 2023

CdS/P25/Ni 2 P were prepared for photocatalytic hydrogen-evolution and simultaneously converting high-concentration of thiols into disulfides with excellent yield under visible-light. A possible mechanism was proposed based on experiment data.

Язык: Английский

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Amine‐Free, Directing‐Group‐Free and Redox‐Neutral α‐Alkylation of Saturated Cyclic Ketones

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(29)

Опубликована: Май 23, 2023

Abstract The activation of the α‐C−H bond ketones typically requires an amine and a directing group to guide reaction selectivity in amine‐catalysis carbonyl chemistry. For ketone, groups are also required control selectivity. Reported herein is first α‐alkylation cyclic absence catalyst group. 1 H NMR, XPS, EPR studies DFT calculations indicate that α‐carbon radical intermediate formed through direct selective inert chelating on surface colloidal quantum dots (QDs). Such interaction essential for weakening C−H bond, as exemplified, using CdSe QDs sole photocatalyst execute alkylation under visible‐light irradiation. Without group, high step‐ atom‐economy transformation redox‐neutral condition opens new way functionalization

Язык: Английский

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Divergent Photosensitizer Controlled Reactions of 4‐Hydroxycoumarins and Unactivated Olefins: Hydroarylation and Subsequent [2+2] Cycloaddition

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(45)

Опубликована: Сен. 26, 2023

Herein, we report a photoinduced approach for hydroarylation of unactivated olefins using 4-hydroxycoumarins as the arylating reagent. Key to success this reaction is conversion nucleophilic into electrophilic carbon radicals via photocatalytic arene oxidation, which not only circumvents polarity-mismatch issue encountered under ionic conditions but also accommodates broad substrate scope and inhibits side reactions that were previously observed. Moreover, divergent reactivity was achieved by changing photocatalyst, enabling subsequent [2+2] cycloaddition deliver cyclobutane-fused pentacyclic products are otherwise challenging access in high yields with diastereoselectivity. Mechanistic studies have elucidated mechanism origin reactivity.

Язык: Английский

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Engineering a molecular ruthenium catalyst into three-dimensional metal covalent organic frameworks for efficient water oxidation

Chemical Science, Год журнала: 2023, Номер 14(42), С. 11768 - 11774

Опубликована: Янв. 1, 2023

Three-dimensional metal covalent organic frameworks (3D MCOFs) were constructed by integrating molecular ruthenium water oxidation catalysts (WOCs) for realizing efficient oxidation.

Язык: Английский

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